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The electrochemical behavior of poly 1-pyrenemethyl methacrylate binder and its effect on the interfacial chemistry of a silicon electrode

Journal Article · · Journal of Power Sources
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  1. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  2. University of Rhode Island, Kingston, RI (United States)

The physico-chemical properties of poly (1-pyrenemethyl methacrylate) (PPy) are presented with respect to its use as a binder in a Si composite anode for Li-ion batteries. PPy thin-films on Si(100) wafer and Cu model electrodes are shown to exhibit superior adhesion as compared to conventional polyvinylidene difluoride (PVdF) binder. Electrochemical testing of the model bi-layer PPy/Si(100) electrodes in a standard organic carbonate electrolyte reveal higher electrolyte reduction current and an overall irreversible cathodic charge consumption during initial cycling versus the uncoated Si electrode. The PPy thin-film is also shown to impede lithiation of the underlying Si. XAS, AFM, TGA and ATR-FTIR analysis indicated that PPy binder is both chemically and electrochemically stable in the cycling potential range however significant swelling is observed due to a selective uptake of diethyl carbonate (DEC) from the electrolyte. The increased concentration of DEC and depletion of ethylene carbonate (EC) at the Si/PPy interface leads to continuous decomposition of the electrolyte and results in non-passivating behavior of the Si(100)/PPy electrode as compared to pristine silicon. Consequently, PPy binder improves the mechanical integrity of composite Si anodes but it influences mass transport at the Si(100)/PPy interface and alters electrochemical response of silicon during cycling in an adverse manner.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
AC02-05CH11231; EE0006443
OSTI ID:
1530331
Alternate ID(s):
OSTI ID: 1496301
Journal Information:
Journal of Power Sources, Journal Name: Journal of Power Sources Journal Issue: C Vol. 376; ISSN 0378-7753
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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